Abstract
Methane (CH4) is a strong greenhouse gas and even though its atmospheric abundance is lower than carbon dioxide (CO2), CH4 has a global warming potential twenty-five times larger than CO2 and its atmospheric abundance has drastically increased since 1800. Understanding the evolution of the CH4 atmospheric abundance is complex, because it is controlled by multiple sources (e.g. wetlands, biomass burning, ruminants, rice paddies and fossil fuel) and sinks, and large uncertainties exist on how sensitive those sources and sinks are to climate variability.
The aim of this research is to understand the influence of climate variability and anthropogenic activity on the CH4 budget, i.e. the balance between the different sources and sinks, during the last two millennia. For this purpose a technique was developed to analyze the CH4 isotopic composition of air in ice cores.
Analysis of the isotopic composition of CH4 preserved in ice cores provides evidence for the environmental drivers of variations in CH4 mixing ratios, because different sources and sinks affect the isotopic composition of CH4 uniquely.
Our main results from air trapped in Greenland ice cores shows that the carbon isotopic composition (d13C) of CH4 underwent pronounced centennial-scale variations between 200 BC and 1600 AD without clear corresponding changes in CH4 mixing ratios. Two-box model calculations suggest that those centennial-scale variations in isotope ratios are due to changes in biomass burning and biogenic sources (e.g. wetlands, agriculture), which are correlated with both natural climate variability, including the Medieval Climate Anomaly and with changes in human population, land-use and important events in history as the expansion of the Roman Empire, the fall of the Han dynasty and the Medieval period. This shows that human activity had an impact on the methane budget already two thousand years ago and is likely responsible for the atmospheric methane increase in the atmosphere during this period.
Also the more recent CH4 budget has been investigated by measuring the isotope composition of CH4 in air trapped in the surface layer of the ice sheet (called "firn"). Several processes involving isotopic fractionation occur in the firn, hence corrections need to be apply to the isotope data in order to reconstruct the atmospheric history. Those corrections were carried out with a firn air transport model and the best-estimate scenario shows an enrichment in d13C of CH4 over the last 50 years very likely caused by enhanced fossil fuel production and consumption during this period.
The role of wetlands, the main natural CH4 source, has also been investigated using measurements of d13C from air trapped in ice covering Arctic lakes in the winter. Those data showed that during the winter and in presence of ice cover, CH4, which is produced in the lake sediment, is partly removed by oxidation in the water column. Therefore, shorter is the period of ice cover on Arctic lakes, more CH4 will reach the atmosphere. This process may be of major importance in a future changing climate.
Original language | English |
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Qualification | Doctor of Philosophy |
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Award date | 22 Jun 2012 |
Print ISBNs | 978-94-6191-338-8 |
Publication status | Published - 22 Jun 2012 |